Unusual Spin Exchanges Mediated by the Molecular Anion P2S64-: Theoretical Analyses of the Magnetic Ground States, Magnetic Anisotropy and Spin Exchanges of MPS3 (M = Mn, Fe, Co, Ni).

ABSTRACT: We examined the magnetic ground states, the preferred spin orientations and the spin exchanges of four layered phases MPS3 (M = Mn, Fe, Co, Ni) by first principles density functional theory plus onsite repulsion (DFT + U) calculations. The magnetic ground states predicted for MPS3 by DFT + U calculations using their optimized crystal structures are in agreement with experiment for M = Mn, Co and Ni, but not for FePS3. DFT + U calculations including spin-orbit coupling correctly predict the observed spin orientations for FePS3, CoPS3 and NiPS3, but not for MnPS3. Further analyses suggest that the ||z spin direction observed for the Mn2+ ions of MnPS3 is caused by the magnetic dipole-dipole interaction in its magnetic ground state. Noting that the spin exchanges are determined by the ligand

SUBMITTER: Koo HJ 

PROVIDER: S-EPMC7961718 | biostudies-literature | 2021 Mar

REPOSITORIES: biostudies-literature